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Synthesis of spherical nano-ZSM-5 zeolite with intergranular mesoporous for alkylation of ethylbenzene with ethanol to produce m-diethylbenzene

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Chinese Journal of Chemical engineering 2024年第3期67卷 298-309页

作者： Siyue Wang Jinhong Li Qingxin Xu Shengjie Song Yu'ni Jiang Lidong Chen Xin Shi Weiguo Cheng Faculty of Chemistry and Chemical engineering Liaoning Normal UniversityDalian 110629China Beijing Key Laboratory of Ionic Liquids Clean process Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Catalytic synthesis of m-diethylbenzene(m-DEB)through alkylation of ethylbenzene(EB)may be a promising alternative route in comparison with traditional rectification of mixed DEB,for which the top priority is to develop efficient and stable heterogeneous catalysts.Here,the spherical nano-ZSM-5 zeolite with abundant intergranular mesoporous is synthesized by the seed-mediated growth method for alkylation of EB with ethanol to produce m-DEB.The results show that the spherical nano-ZSM-5 zeolite exhibits better stability and higher alkylation activity at a lower temperature than those of commercial micropore ZSM-5.And then,the spherical nano-ZSM-5 is further modified by La_(2)O_(3) through acid treatment followed by immersion method.The acid treatment causes nano-ZSM-5 to exhibit the increased pore size but decreased the acid sites,and subsequent La_(2)O_(3) loading reintroduces the weak acid sites.As a result,the HNO_(3)-La_(2)O_(3)-modified catalyst exhibits a slight increase in EB conversion and DEB yield in comparison with unmodified one,and meanwhile,it still maintains high m-DEB selectivity.The catalyst after acid treatment achieves higher catalytic stability besides maintaining the high alkylation activity of EB with ethanol.The present study on the spherical nano-HZSM-5 zeolite and its modification catalyst with excellent alkylation ability provides new insights into the production of mDEB.

关键词： Zeolite Modification Alkylation reaction m-diethylbenzene Catalyst Fixed-bed

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Alternative technology for the recovery of butyl acetate with low concentration:high capacity adsorbent and high efficiency adsorption

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Green Chemical engineering 2024年第2期5卷 236-244页

作者： Chi Ma Lihong Zhao Zhengxin Mao Hao Su Qingfen Liu CAS Key Laboratory of Green process and engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical engineering University of Chinese Academy of SciencesBeijing100049China

Industrial pharmaceutical wastewater usually contains butyl acetate(BA)with a concentration of 1 wt%-7 wt%,and the traditional method for BA recovery is distillation with high energy consumption.Adsorption method is developed to recover BA with low concentration for the high efficiency and low energy consumption.Medium polar polyacrylate resins with macroporous structure of 233.1 nm and average particle size of about 526.5μm are successfully synthesized by suspension polymerization and used for the BA adsorption and desorption.The maximum adsorption capacity reaches 171.1 mg g^(-1)with relative standard deviation(RSD)value of 0.2%,which is more than twice the results in the literature.The BA desorption rate is 97.0%at 100℃with RSD value of 0.4%,and the resins are beneficial to the reuse in the adsorption-desorption cycle.The adsorption thermodynamics and kinetics are investigated,and the BA adsorption is a spontaneous and endothermic process with the increase of disorder degree.This process is mainly contributed by physical absorption and agree well with Freundlich model and pseudo-first-order adsorption kinetic model.The adsorption method avoids boiling a large amount of wastewater and hopefully provides a novel alternative technology for the BA recovery.

关键词： Butyl acetate recovery Resin adsorption Desorption Thermodynamics Kinetics

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Promoting effect of FeOx addition on the mechanochemically prepared vanadium-based catalyst for real PCDD/Fs removal and mechanism insight

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Journal of Environmental Sciences 2024年第3期137卷 478-487页

作者： Minghui Tang Ling Wang Hongxian Li Xinlei Huang Cuicui Du Shengyong Lu State Key Laboratory for Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou 310027China

Industrial-use VOx-based catalysts usually have a higher active temperature window (>250-300℃),which becomes a“bottleneck”for the practical application of PCDD/Fs catalytic degradation technology.In this work,VO_(x)-FeO_(x)/TiO_(2) catalyst prepared via mechanochemically method was investigated for the catalytic removal of PCDD/Fs.The removal efficiency of 1,2-DCBz,pure PCDD/Fs gas generated in the lab,PCDD/Fs from actual fue gas,long-term were studied,and the degradation mechanism was explored using FTIR and TOFMS.The degradation efficiency of 1,2-DCBz and PCDD/Fs on VO_(x)-FeO_(x)/TiO_(2) were higher than that of VO_(x)/TiO_(2)catalyst,and the optimal FeOx addition ratio was 3 wt.%.The characterization results show that the addition of FeOx can effectively improve the pore structure,surface acidity,and VOx dispersion of the catalyst,thus contributing to increasing the V^(5+)content and surface-active oxygen,which is conducive to the improvement of adsorption and redox performance of the catalyst.Under the actual MSWI (municipal solid waste incineration)fue gas,the PCDD/Fs removal efficiency over VTi-3Fe-MC maintained long-term stability,higher than 85%for 240 min.This result was not significantly reduced compared with the data obtained in the laboratory.According to the analysis results of intermediate products by FTIR and GC-TOFMS,it can be inferred that the epoxidation fracture of benzene ring is the rate-limiting step of dioxin catalytic degradation reaction.This work gives an in-depth view into the PCDD/Fs removal over VO_(x)-FeO_(x)/TiO_(2) catalysts and could provide guidelines for the rational design of reliable catalysts for industrial applications.

关键词： PCDD/F removal MSWI fue gas VO_(x)-FeO_(x)/TiO_(2) Mechanochemical GC-TOFMS

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Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu Beijing Key Laboratory of Ionic Liquids Clean process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences University of Chinese Academy of Sciences

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of resources.In this work,a strategy of lanthanum manganese mixed metal oxides(LMMO) regulated via a facile ionic liquid (IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of cyclohexane.An 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone) selectivity was achieved over the optimal LMMO catalyst under mild conditions.The effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional catalysts.The formation of self-assembled spherical nanoparticles followed the‘‘dissolution-nucleation-proliferation’’mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal environment.Importantly,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) and radical trapping experiments.The recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： Ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

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A projected Newton algorithm based on chemically allowed interval for chemical equilibrium computations

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Frontiers of Chemical Science and engineering 2024年第3期18卷 25-37页

作者： Hongbin Lu Shaohui Tao Xiaoyan Sun Li Xia Shuguang Xiang Institute of process Systems engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China

The chemical equilibrium equations utilized in reactive transport modeling are complex and nonlinear,and are typically solved using the Newton-Raphson method.Although this algorithm is known for its quadratic convergence near the solution,it is less effective far from the solution,especially for ill-conditioned problems.In such cases,the algorithm may fail to converge or require excessive iterations.To address these limitations,a projected Newton method is introduced to incorporate the concept of projection.This method constrains the Newton step by utilizing a chemically allowed interval that generates feasible descending iterations.Moreover,we utilize the positive continuous fraction method as a preconditioning technique,providing reliable initial values for solving the algorithms.The numerical results are compared with those derived using the regular Newton-Raphson method,the Newton-Raphson method based on chemically allowed interval updating rules,and the bounded variable least squares method in six different test cases.The numerical results highlight the robustness and efficacy of the proposed algorithm.

关键词： chemical equilibrium reactive transport modeling numerical methods projected Newton method

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Effects of the inlet particle spatial distribution on the performance of a gas-solid cyclone separator

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Particuology 2024年第2期85卷 133-145页

作者： Yuge Yao Manxia Shang Xiwei Ke Zhong Huang Tuo Zhou Junfu Lyu Key Laboratory for thermal Science and Power engineering of Ministry of Education Department of Energy and Power EngineeringTsinghua UniversityBeijing100084China

The present study was aimed at the inlet particle spatial distribution of a gas-solid separator with high solid loading and investigated its effects on cyclone performance and the inner flow pattern.The flow fields of a cyclone with different rectangular particle flow areas on the inlet surface were numerically simulated using a four-way coupling method.The simulated results indicate that reducing the inlet particle flow area and lowing the inlet particle position can effectively reduce the scattered particles inside the cyclone separator and enhance the separation performance.Vertically gathering the particles to the centerline can also weaken the particle back-mixing.The particles near the roof account for the swirling particle ceiling phenomenon.The inlet particle spatial distribution affects the pressure drop mainly by affecting the gas tangential velocity in the cylinder body.Moreover,compared to the hori-zontal particle distribution on the inlet surface,the vertical particle distribution has greater effects on cyclone performance.

关键词： Gas-solid cyclone Inlet particle spatial distribution Four-way coupling Separation efficiency Scattered particle

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Selective cyclohexane oxidation enhancement by electronic structures regulation of metal-poly(ionic liquid)s

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Green Chemical engineering 2024年第2期5卷 213-221页

作者： Ying Jin Shengxin Chen Ruirui Wang Yumei Liu Xinxin Li Yingwei Li Ruirui Zhang Ruixia Liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou450001China Beijing Key Laboratory of Ionic Liquids Clean process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringInnovation Academy for Green ManufactureCASBeijing100190China

Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in catalysis.In this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of cyclohexane.Characterization analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial catalysts.Compared with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil yield.More interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the catalyst.Therefore,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.

关键词： Metal-PILs Cyclohexane oxidation C-H activation Co-N sites

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Three-stage pyrolysis–steam reforming–water gas shift processing of household,commercial and industrial waste plastics for hydrogen production

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Waste Disposal and Sustainable Energy 2024年第1期6卷 25-37页

作者： Rayed Alshareef Robert Sait-Stewart Mohamad A.Nahil Paul T.Williams School of Chemical and process engineering University of LeedsLeedsLS29JTUK

Five common single plastics and nine different household,commercial and industrial waste plastics were processed using a three-stage(i)pyrolysis,(ii)catalytic steam reforming and(iii)water gas shift reaction system to produce hydrogen.Pyrolysis of plastics produces a range of different hydrocarbon species which are subsequently catalytically steam reformed to produce H_(2)and CO and then undergo water gas shift reaction to produce further H_(2).The process mimics the commercial process for hydrogen production from natural gas.processing of the single polyalkene plastics(high-density polyethylene(HDPE),low-density polyethylene(LDPE),and polypropylene(PP))produced similar H_(2)yields between 115 mmol and 120 mmol per gram plastic.Even though PS produced an aromatic product slate from the pyrolysis stage,further stages of reforming and water gas shift reaction produced a gas yield and composition similar to that of the polyalkene plastics(115 mmol H_(2)per gram plastic).PET gave significantly lower H_(2)yield(41 mmol per gram plastic)due to the formation of mainly CO,CO_(2)and organic acids from the pyrolysis stage which were not conducive to further reforming and water gas shift reaction.A mixture of the single plastics typical of that found in municipal solid waste produced a H_(2)yield of 102 mmol per gram plastic.Knowing the gas yields and composition from the single plastics enabled an estimation of the yields from a simulated waste plastic mixture and a‘real-world’waste plastic mixture to be determined.The different household,commercial and industrial waste plastic mixtures produced H_(2)yields between 70 mmol and 107 mmol per gram plastic.The H_(2)yield and gas composition from the single waste plastics gave an indication of the type of plastics in the mixed waste plastic samples.

关键词： Waste plastic Hydrogen Catalyst Pyrolysis reforming Water gas shift

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A comprehensive review on microchannel heat sinks for electronics cooling

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International Journal of Extreme Manufacturing 2024年第2期6卷 133-162页

作者： Zhi-Qiang Yu Mo-Tong Li Bing-Yang Cao Key Laboratory for thermal Science and Power engineering of Ministry of Education Department of Engineering MechanicsTsinghua UniversityBeijing 100084People’s Republic of China

The heat generation of electronic devices is increasing dramatically,which causes a serious bottleneck in the thermal management of electronics,and overheating will result in performance deterioration and even device damage.With the development of micro-machining technologies,the microchannel heat sink(MCHS)has become one of the best ways to remove the considerable amount of heat generated by high-power electronics.It has the advantages of large specific surface area,small size,coolant saving and high heat transfer coefficient.This paper comprehensively takes an overview of the research progress in MCHSs and generalizes the hotspots and bottlenecks of this area.The heat transfer mechanisms and performances of different channel structures,coolants,channel materials and some other influencing factors are reviewed.Additionally,this paper classifies the heat transfer enhancement technology and reviews the related studies on both the single-phase and phase-change flow and heat transfer.The comprehensive review is expected to provide a theoretical reference and technical guidance for further research and application of MCHSs in the future.

关键词： microchannel heat sink thermal management of electronics microscale heat transfer heat transfer enhancement

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Observation of ballistic-diffusive thermal transport in GaN transistors using thermoreflectance thermal imaging

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Rare Metals 2024年第1期43卷 389-394页

作者： Zhi-Ke Liu Yang Shen Han-Ling Li Bing-Yang Cao Key Laboratory for thermal Science and Power engineering of Ministry of Education Department of Engineering MechanicsTsinghua UniversityBeijing 100084China

To develop effective thermal management strategies for gallium-nitride (GaN) transistors, it is essential to accurately predict the device junction temperature. Since the width of the heat generation in the devices is comparable to phonon mean free paths (MFPs) of GaN, phonon ballistic transport exists and can significantly affect the heat transport process.

关键词： temperature. transistors GaN

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